Malhotra replaces Paul McFarland, who departed Toronto for a head coaching gig with the OHL's Kingston Frontenacs.
The 40-year-old has been with the Vancouver Canucks organization since 2016 when the team hired him as a development coach. The Canucks promoted him to assistant coach in 2017.
"I'm very grateful to the Canucks organization for the opportunity given to me to start my coaching career. It was truly a great experience to learn from Travis Green and the rest of his staff," Malhotra said. "I'm now very excited for this opportunity with the Leafs moving forward - to be working with Sheldon, his staff, and this young, talented team."
Malhotra, a Mississauga, Ontario, native, played 991 NHL games and totaled 116 goals and 179 assists. The veteran was well-known during his career for his two-way abilities and proficiency at faceoffs.
He finished his tenure with a 56.4 winning percentage in the faceoff circle. During the 2019-20 regular season, Vancouver ranked second in the league in faceoffs with a 54% win rate.